The rapid growth in nuclear industries such as uranium ores mining, nuclear energy generation, spent-fuel treatment and nuclear weapon manufacture has caused a legacy of uranium contamination in the ...aquatic environment, which poses a potential threat to the ecological environment and human health. The safe and effective disposal of uranium-contaminated water has thus been an urgent requirement. For decades, various materials have been shown to be capable for removing uranium from aqueous solution by adsorption technique, namely inorganic materials (e.g., clay minerals, metal oxides, mesoporous silica), organic polymers (e.g., resins, cellulose, chitosan), carbon family materials (e.g., mesoporous carbon, carbon nanotubes, graphene oxides), and porous framework materials (e.g., covalent organic frameworks, metal-organic frameworks). In this review, we provide a systematic and comprehensive overview of the researches conducted from 2005 to 2018 for uranium removal from aqueous solution by these emerging materials. The different approaches in the determination of the adsorption mechanisms between uranium and adsorbents are also briefly summarized, involving macroscopic experimental approaches, microscopic spectroscopic and computational approaches. Finally, we discuss the current limitations and propose future research perspectives in hopes of inspiring more dramatic advancements in the material and environment remediation fields.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
•Sorption and in-situ reduction of U(VI) is observed.•The composites are more effective for U(VI) removal and solidification.•The inner-sphere surface complexes are observed.
The reduced graphene ...oxide-supported nanoscale zero-valent iron (nZVI/rGO) composites were synthesized by chemical deposition method and were characterized by SEM, high resolution TEM, Raman and potentiometric acid-base titrations. The characteristic results showed that the nZVI nanoparticles can be uniformly dispersed on the surface of rGO. The removal of U(VI) on nZVI/rGO composites as a function of contact time, pH and U(VI) initial concentration was investigated by batch technique. The removal kinetics of U(VI) on nZVI and nZVI/rGO were well simulated by a pseudo-first-order kinetic model and pseudo-second-order kinetic model, respectively. The presence of rGO on nZVI nanoparticles increased the reaction rate and removal capacity of U(VI) significantly, which was attributed to the chemisorbed OH− groups of rGO and the massive enrichment of Fe2+ on rGO surface by XPS analysis. The XRD analysis revealed that the presence of rGO retarded the transformation of iron corrosion products from magnetite/maghemite to lepidocrocite. According to the fitting of EXAFS spectra, the UC (at ∼2.9Å) and UFe (at ∼3.2Å) shells were observed, indicating the formation of inner-sphere surface complexes on nZVI/rGO composites. Therefore, the nZVI/rGO composites can be suitable as efficient materials for the in-situ remediation of uranium-contaminated groundwater in the environmental pollution management.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Adsorption of 4-n-nonylphenol (4-n-NP) and bisphenol A (BPA) on magnetic reduced graphene oxides (rGOs) as a function of contact time, pH, ionic strength and humic acid were investigated by batch ...techniques. Adsorption of 4-n-NP and BPA were independent of pH at 3.0- 8.0, whereas the slightly decreased adsorption was observed at pH 8.0–11.0. Adsorption kinetics and isotherms of 4-n-NP and BPA on magnetic rGOs can be satisfactorily fitted by pseudo-second-order kinetic and Freundlich model, respectively. The maximum adsorption capacities of magnetic rGOs at pH 6.5 and 293 K were 63.96 and 48.74 mg/g for 4-n-NP and BPA, respectively, which were significantly higher than that of activated carbon. Based on theoretical calculations, the higher adsorption energy of rGOs + 4-n-NP was mainly due to π–π stacking and flexible long alkyl chain of 4-n-NP, whereas adsorption of BPA on rGOs was energetically favored by a lying-down configuration due to π–π stacking and dispersion forces, which was further demonstrated by FTIR analysis. These findings indicate that magnetic rGOs is a promising adsorbent for the efficient elimination of 4-n-NP/BPA from aqueous solutions due to its excellent adsorption performance and simple magnetic separation, which are of great significance for the remediation of endocrine-disrupting chemicals in environmental cleanup.
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The effect of Cr(VI) and bisphenol A (BPA) on U(VI) photoreduction by C3N4 photocatalyst was demonstrated by the batch experiments, electron spin resonance (ESR), X-ray photoelectron spectroscopy ...(XPS), X-ray absorption near edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) techniques. The batch experiments manifested that Cr(VI) and BPA enhanced the photocatalytic activity of C3N4 for U(VI) photoreduction, whereas U(VI) photoreduction was significantly diminished with increased pH from 4.0 to 8.0. According to radical scavengers and ESR analysis, U(VI) was photoreduced to U(IV) by photogenerated electrons of conduction band edge, whereas Cr(VI) was reduced to Cr(III) by H2O2. BPA and its products such as organic acid and alcohols can capture photoinduced holes, which resulted in the enhancement of U(VI) photoreduction to U(IV). XPS and XANES analyses demonstrated that U(VI) was gradually photoreduced to U(IV) by C3N4 within irradiation 60 min, whereas U(IV) was reoxidized to U(VI) with increasing irradiation time. EXAFS analysis determined that the dominant interaction mechanisms of U(VI) on C3N4 after irradiation for 240 min were reductive precipitation and inner-sphere surface complexation. This work highlights the synergistic removal of radionuclides, heavy metals, and persistent organic pollutants by C3N4, which is crucial for the design and application of a high-performance photocatalyst in actual environmental cleanup.
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Carbon-based nanomaterials, especially carbon nanotubes and graphene, have drawn wide attention in recent years as novel materials for environmental applications. Notably, the functionalized ...derivatives of carbon nanotubes and graphene with high surface area and adsorption sites are proposed to remove heavy metals via adsorption, addressing the pressing pollution of heavy metal. This critical revies assesses the recent development of various functionalized carbon nanotubes and graphene that are used to remove heavy metals from contaminated water, including the preparation and characterization methods of functionalized carbon nanotubes and graphene, their applications for heavy metal adsorption, effects of water chemistry on the adsorption capacity, and decontamination mechanism. Future research directions have also been proposed with the goal of further improving their adsorption performance, the feasibility of industrial applications, and better simulating adsorption mechanisms.
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•Removal of heavy metals from water has drawn wide attention.•Various functionalized carbon nanotube and graphene nanomaterials were stated.•Effects of water environmental chemistry on heavy metals removal were discussed.•Adsorption isotherms, kinetics, thermodynamics, and pathways were discussed.•Some research prospects were proposed for future studies and application.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Clay minerals have been proposed for the potential retention of the high-level radioactive wastes in deep geological repositories. The retention of uranium (U(VI)) and europium (Eu(III)) onto ...well-characterized sepiolite was elucidated by using microscopic adsorption, spectroscopic techniques and surface complexation modeling. The results of macroscopic adsorption experiments showed that the uptake of U(VI) and Eu(III) onto sepiolite significantly increased with increasing pH 4.0–7.0, whereas the decrease adsorption of U(VI) at pH>7.0 and in the presence of carbonate (10−3mol/L) was attributed to the electrostatic repulsion. The chemical affinity of U(VI) with sepiolite was stronger than that of Eu(III) with sepiolite in terms of batch desorption tests. Based on the EXAFS spectra analysis, the interatomic distances of U–Si at ∼3.16Å was observed in U(VI)/sepiolite systems, which indicated that the inner-sphere surface species were coordinated on SiO4 tetrahedra via bidentate configuration. The U–C shell at ∼2.9Å in the presence of carbonate revealed the U(VI)-carbonate ternary complexes at sepiolite–water interface. The results from the three common surface complexation models (SCMs), including constant-capacitance model (CCM), diffuse-layer model (DLM), and triple-layer model (TLM), can give an excellent fit to the experimental data with the bidentate edge-sharing (E2, >SO2M(n−2)+), bidentate corner-sharing (C2, (>SO)2M(OH)2(n−4)+) and >SOMCO3(n−3)+ inner-sphere surface complexes in ambient environments. However, the second ternary surface complex >SOCO2M(n−1)+ was determined in the presence of carbonate. The findings presented in this study are significant toward the description and predication of fate and transport of radionuclides at the water–mineral interface in the natural environment.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
During the latest several decades, the continuous development of the economy and industry has brought more and more serious organic pollutants to the natural environment, which have inevitably ...aroused severe menace to human health and the environmental system. The nano zero-valent iron (NZVI) particles and NZVI-based materials have widely applied to remove organic pollutants. This article reviews the key advancements of different methods for the synthesis of NZVI and NZVI-based materials. Different modification methods (e.g., doped NZVI, encapsulated NZVI and supported NZVI) are also introduced detailedly for overcoming the defects of NZVI such as aggregation and easy oxidation. The removal of different organic pollutants including dyes, halogenated organic compounds, nitro-organic compounds, phenolic compounds, pesticides, and antibiotics are summarized. The interaction mechanisms, including adsorption, reduction, and active oxidation of organic pollutants by NZVI/NZVI-based composites, are discussed. The dyes are mainly removed by destroying their chromogenic group according to the reduction or the Fenton-like reaction with NZVI. The removal of halogenated organic compounds (HOCs) is realized by the dehalogenation process, including reductive elimination, hydrogenolysis, and hydrogenation. As for the nitro-organic compounds, three different reduction pathways as nitro-reduction (into amino), cleavage at the carbon‑nitrogen bond or denitration of the NO2 group may take effect. The phenolic compounds can be mineralized into inorganic molecules, including CO2 and H2O, by Fenton oxidation. This review might provide the basis for future studies on developing more effective NZVI-based materials for the treatment of wastewaters contaminated by organic pollutants.
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•Synthesis and modification of NZVI and NZVI-based composites were summarized.•Removal of organic pollutants by NZVI and NZVI-based composites were reviewed and compared.•The interaction mechanism was discussed from spectroscopy analysis and theoretical calculation.•The challenges and perspectives for NZVI-based composites were discussed.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Highly efficient removal of metal ion pollutants, such as toxic and nuclear waste-related metal ions, remains a serious task from the biological and environmental standpoint because of their harmful ...effects on human health and the environment. Recently, highly porous metal-organic frameworks (MOFs), with excellent chemical stability and abundant functional groups, have represented a new addition to the area of capturing various types of hazardous metal ion pollutants. This review focuses on recent progress in reported MOFs and MOF-based composites as superior adsorbents for the efficient removal of toxic and nuclear waste-related metal ions. Aspects related to the interaction mechanisms between metal ions and MOF-based materials are systematically summarized, including macroscopic batch experiments, microscopic spectroscopy analysis, and theoretical calculations. The adsorption properties of various MOF-based materials are assessed and compared with those of other widely used adsorbents. Finally, we propose our personal insights into future research opportunities and challenges in the hope of stimulating more researchers to engage in this new field of MOF-based materials for environmental pollution management.
Metal-organic framework-based materials represent a new addition to the area of capturing diverse toxic and radioactive metal ions.
Graphene oxide-supported polyaniline (PANI@GO) composites were synthesized by chemical oxidation and were characterized by SEM, Raman and FT-IR spectroscopy, TGA, potentiometric titrations, and XPS. ...The characterization indicated that PANI can be grafted onto the surface of GO nanosheets successfully. The sorption of U(VI), Eu(III), Sr(II), and Cs(I) from aqueous solutions as a function of pH and initial concentration on the PANI@GO composites was investigated. The maximum sorption capacities of U(VI), Eu(III), Sr(II), and Cs(I) on the PANI@GO composites at pH 3.0 and T = 298 K calculated from the Langmuir model were 1.03, 1.65, 1.68, and 1.39 mmol·g–1, respectively. According to the XPS analysis of the PANI@GO composites before and after Eu(III) desorption, nitrogen- and oxygen-containing functional groups on the surface of PANI@GO composites were responsible for radionuclide sorption, and that radionuclides can hardly be extracted from the nitrogen-containing functional groups. Therefore, the chemical affinity of radionuclides for nitrogen-containing functional groups is stronger than that for oxygen-containing functional groups. This paper focused on the application of PANI@GO composites as suitable materials for the preconcentration and removal of lanthanides and actinides from aqueous solutions in environmental pollution management in a wide range of acidic to alkaline conditions.
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The presence of heavy metals in the industrial effluents has recently been a challenging issue for human health. Efficient removal of heavy metal ions from environment is one of the most important ...issues from biological and environmental point of view, and many studies have been devoted to investigate the environmental behavior of nanoscale zerovalent iron (NZVI) for the removal of toxic heavy metal ions, present both in the surface and underground wastewater. The aim of this review is to show the excellent removal capacity and environmental remediation of NZVI-based materials for various heavy metal ions. A new look on NZVI-based materials (e.g., modified or matrix-supported NZVI materials) and possible interaction mechanism (e.g., adsorption, reduction and oxidation) and the latest environmental application. The effects of various environmental conditions (e.g., pH, temperature, coexisting oxy-anions and cations) and potential problems for the removal of heavy metal ions on NZVI-based materials with the DFT theoretical calculations and EXAFS technology are discussed. Research shows that NZVI-based materials have satisfactory removal capacities for heavy metal ions and play an important role in the environmental pollution cleanup. Possible improvement of NZVI-based materials and potential areas for future applications in environment remediation are also proposed.
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